III International Conference

PP-I-32STEAM AND AUTOTHERMAL REFORMING OF METHANE OVER NICKELCATALYST: EXPERIMENT, MODELING, AND NUMERICAL SIMULATIONMaier L., Schädel B., Deutschmann O.Institute for Chemical Technology and Polymer Chemistry, University of Karlsruhe, GermanyE-mail: maier@ict.uni-karlsruhe.deThe kinetics of steam and autothermal reforming of methane over nickel coated monolithcatalyst were investigated experimentally and numerically. A multi-step heterogeneousreaction mechanism for partial oxidation and steam reforming of methane including thereverse water-gas shift reaction and methanation was developed to analyze the kinetic data.DETCHEM computational tool that use two-dimensional boundary-layer approximationincluding detailed models for heterogeneous reactions as well as transport phenomena wasused for the numerical investigation. The gas composition and surface coverage withadsorbed species were calculated as function of the position in the monolith. The numericalsimulation of conversions and selectivities are shown and compared with experimental values.The model and surface reaction mechanism developed are able to properly describe bothsteam and autothermal reforming of methane on Ni catalysts at the wide range of temperatureand steam/methane ratio.Steam reforming of methane has been the most widely used industrial process for thesynthesis gas production. For many years, partial oxidation (POX) and CO 2 reforming ofnatural gas to synthesis gas have attracted much interest because of their potential to reducethe cost of synthesis gas and for application in chemical energy storage and transmissiontechnology [1]. Recently, also the internal reforming in the anode of a solid oxide fuel cells(SOFC) operated with hydrocarbons has been extensively discussed [2]. Modeling ofautothermal reforming of natural gas to synthesis gas, where both steam and oxygen arepresent in the feed gas demands the combination of reaction schemes of reforming as well aspartial and total oxidation [3].The kinetics of steam and autothermal reforming of methane over nickel coated monolithcatalyst were investigated experimentally and numerically. A multi-step heterogeneousreaction mechanism for partial oxidation and steam reforming of methane including thereverse water-gas shift and methanation reactions was developed. The surface reactionmechanism consisting of 42 reactions among 7 stable gas-phase and further 14 adsorbedspecies was coupled with an elementary step gas phase reaction mechanism and twodimensionalflow models to describe the catalytic reactor applied. The numerical simulationsof the reforming process at various conditions were performed using the CFD codeDETCHEM CHANNEL [4].65